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AU600248B2 - N- (butenyl-substituted) azaheterocyclic carboxylic acids - Google Patents
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AU600248B2 - N- (butenyl-substituted) azaheterocyclic carboxylic acids - Google Patents

N- (butenyl-substituted) azaheterocyclic carboxylic acids Download PDF

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AU600248B2
AU600248B2 AU67193/87A AU6719387A AU600248B2 AU 600248 B2 AU600248 B2 AU 600248B2 AU 67193/87 A AU67193/87 A AU 67193/87A AU 6719387 A AU6719387 A AU 6719387A AU 600248 B2 AU600248 B2 AU 600248B2
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Ursula Sonnewald
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Novo Nordisk AS
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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D401/00Heterocyclic compounds containing two or more hetero rings, having nitrogen atoms as the only ring hetero atoms, at least one ring being a six-membered ring with only one nitrogen atom
    • C07D401/02Heterocyclic compounds containing two or more hetero rings, having nitrogen atoms as the only ring hetero atoms, at least one ring being a six-membered ring with only one nitrogen atom containing two hetero rings
    • C07D401/06Heterocyclic compounds containing two or more hetero rings, having nitrogen atoms as the only ring hetero atoms, at least one ring being a six-membered ring with only one nitrogen atom containing two hetero rings linked by a carbon chain containing only aliphatic carbon atoms
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61PSPECIFIC THERAPEUTIC ACTIVITY OF CHEMICAL COMPOUNDS OR MEDICINAL PREPARATIONS
    • A61P25/00Drugs for disorders of the nervous system
    • A61P25/08Antiepileptics; Anticonvulsants
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D405/00Heterocyclic compounds containing both one or more hetero rings having oxygen atoms as the only ring hetero atoms, and one or more rings having nitrogen as the only ring hetero atom
    • C07D405/02Heterocyclic compounds containing both one or more hetero rings having oxygen atoms as the only ring hetero atoms, and one or more rings having nitrogen as the only ring hetero atom containing two hetero rings
    • C07D405/06Heterocyclic compounds containing both one or more hetero rings having oxygen atoms as the only ring hetero atoms, and one or more rings having nitrogen as the only ring hetero atom containing two hetero rings linked by a carbon chain containing only aliphatic carbon atoms
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D409/00Heterocyclic compounds containing two or more hetero rings, at least one ring having sulfur atoms as the only ring hetero atoms
    • C07D409/02Heterocyclic compounds containing two or more hetero rings, at least one ring having sulfur atoms as the only ring hetero atoms containing two hetero rings
    • C07D409/06Heterocyclic compounds containing two or more hetero rings, at least one ring having sulfur atoms as the only ring hetero atoms containing two hetero rings linked by a carbon chain containing only aliphatic carbon atoms

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  • Plural Heterocyclic Compounds (AREA)
  • Acyclic And Carbocyclic Compounds In Medicinal Compositions (AREA)

Description

01- i 0 1-1 0 248 FORM 10 SPRUSON &8 FERGUSON COMMONWEALTH OF AUSTRALIA PATENTS ACT 1952 COMPLETE SPECIFICAT!ON
(ORIGINAL)
FOR OFFICE USE: Class Int. Class Complete Specification Lodged: Accepted: a o z,0 Published: Priority: Related Art: Thi! ometnt contains the Sar.er.ts made i" 1 1 r ii'i Name of Applicant: Address of Applicant: Actual Inventor: Address for Service: Novo Industri A/S Novo Alle, 2880 Bagsvaerd, Denmark URSULA SONNEWALD Spruson Ferguson, Patent Attorneys, Level 33 St Martins Tower, 31 Market Street, Sydney, New South Wales, 2000, Australia Complete Specification for the invention entitled: N fuI- +uACdt) q k eipcyc ic CarE-c Ic-W The following statement is a full description of this invention, including the best method of, performing it known to us SBR:JMA:220W TON/VMN, 1986-12-16, 3o, D-363, IL 3020.200 00 00 0 0 o 0 0 0000 0 o 00 0 000000 o 0 00 0 0 0000 0 OU 0 000 0 00 0 g0o 0 0a a 00 t&s- (t3u-ery su zvlc)aqhetry ca.rboq(cyi c( I-, P oe4~R i ei Dr- at1
ABSTRACT
Phenylbutene derivatives having optionally substituted phenyl and pyrrolyl, furanyl, pyridinyl, pyrazinyl, irnidazolyl, pyrazolyl, pyrimidinyl, pyrrolidinyl, tetrahydrofuranyl, piperidinyl, piperazinyl or alkyithienyl in the 4-position and 3-carboxypiperid-1-yl, 3carboxytetrahydropyrid-l-yl or 3-carboxyrnethylpyrrolidin-l-yl in the 1-position potentiate GABA'ergic neurotransmissioni.
E:
1A SUMMARY OF THE INVENTION The present Invention relates to phenylbuten derivatives of the general formula I
R
1
-C-CH-CH
2
-CH
2
-R
3
(I)
12
R
wherein R represents phenyl optionally substituted by one, two or more substituents selected from the group consisting of halogen, lower alkyl, and lower alkoxy, R 2 represents pyrrolyl, furanyl, pyridinyl, pyrazinyl, imidazolyl, pyrazolyl, pyrimidinyl, pyrrolidinyl, tetrahydrofuranyl, piperidinyl or piperazinyl each of which may be substituted by one, two or 0o oo more substituents selected from the group consisting of halogen, lower 00 2 o0.o alkyl and lower alkoxy or R represents a thienyl group substituted by a 0 0 0 o° loweralkyl group which substituted thienyl group may be further substituted 000000 o 0 o by one, two or more substituents selected from the group consisting of 00 o0,15 halogen, lower alkyl, and lower alkoxy, and R represents 0 o°0 3-carboxypiperid-l-yl, 3-carboxy-l ,2,5,6-tetrahydropyrid-l-yl or 0000 3-carboxymethylpyrrolidin-l-yl, the corresponding amides or lower alkyl esters, or salts thereof. The compounds have interesting and valuable pharmacological properties.
o0: 20 BACKGROUND OF THE INVENTION 048 In the last decade, intensive pharmacological research concerning y-aminobutyric acid (hereinafter designated GABA), a neurotransmitter in the central nervous system, has taken place.
Increased GABA'ergic activity is useful in the treatment of anxiety, pain, epilepsy and muscular and movement disorders. Furthermore, these compounds can be used as sedatives.
511U ToN/VMN, 1986-12-16, 3o, D-363, ILII\, 3020.200 In U.S. patent specification No. 4,383,999 (Srithkline Beckmann Corporation) some derivatives of N-(4phenyl-3-butenyl)azaheterocyclic carboxylic acids which have, furthermore, inter alia, phenyl, p-fluorophenyl, cyclohexyl or thienyl in the 4- position, are described.
According to J.Pharm.Exp.Therap. 228 (1984), 109 et seq., N-(4,4-diphenyl--3-butenyl)nipecotic acid (designated SK&F 89976A), N-(4,4-diphenyl-3-butenyl)guvacine (designated SK&F 100330A), N-(4,4-diphenyl-.3-butenyl)-f3-homoproline (designated SK&F 100561) and N-(4--phenyl-4-(2-thienyl)-3-butenyl)nipecotic acid (designated SI &F 100604J) are orally active inhibitors of GABA uptake.
00000 ao0 00 0 0 DETAILED PRACTICE OF THIS INVENTION 00 0000 It has now been found that novel compounds of the general formula I stated in Claim 1, below, exhibit GABA uptake 0n 0 0 inhibitory properties and possess useful pharmacological 0 o~ properties on the central nervous system, a selective enhancement of GABA activity. Surprisingly, these effects are 0 V 4superior to those of previously known compounds. Compounds of formula I may be used for -treatment of, for example, pain, anxiety, epilepsy, certain muscular and movement disorders and o other neurological disorders and as sedatives and hypnotics.
Herein pyrroly. is 2-pyrrolyl or 3-pyrrolyl, furanyl is 2-furanyl or 3-furanyl, pyridinyl (pyridyl) is 2-pyridyl, 3-pyridyl or 4-pyridyl, pyrazinyl is 2-pyrazinyl or 3pyrazinyl.. imidazolyl is 2-imidazolyl, 4-imidazolyl or imidazolyl, pyrazolyl is 3-pyrazolyl, 4-pyrazolyl or pyrazolyl, pyrimidinyl is 2-pyrimidinyl, 4-pyriridinyl, pyrimidinyl or 6-pyrimidinyl, pyrrolidinyl is 2"-pyrrolidinyl or 3-pyrrolidinyl, te-trahydrofuranyl is 2-tetrahydrofuranyl or 3tetrahydrofuranyl, piperidinyl (piperidyl) is 2-piperidyl, 3piperidyl or 4-piperidyl, piper"azinyl is 2-piperazinyl, 3piperazinyl or 4-piperazinyl and thienyl is 2-thienyl or 3- ToN/VMN, 1986-12-16, 3o, D-363, IL 3020.200 thianyl. Furthermore, halogen is, preferably, chioro, bromo and fluoro. The lower alkyl group contains less than 8 carbon atoms, preferably less than 5 carbon atoms, and some preferred alkyl groups are methyl and ethyl. The lower alkoxy group contains less than 8 carbon atoms, preferably less than carbon atoms, and some prfered alko/xy gro ps are methoxy and ethoxy. Preferably, i-c-wer alk.'l)h~y is 3-met~hylthien-2-yl.
Specific examples of substituted groups R 1and R 2are Nmethylpyrrol-2-yl and N-methylpyrrol-3-yl.
Compounds of formula I are, for example: 00 00 0 0' N-(4-(N-methylpyrrol-2-.yl)-4-phenylbut-3-en-l-yl)nipecotic 0 0 acid, O 0 a N-(4-(N-methylpyrrol-2-yl)--4-phenylbut-3-en-l-yl)guvacine, 0 0 N-(4-(N-methylpyrrol-2-yl)-4-phenylbut-3-en-1-yl)-8ho0or0ie 0 00 0001D N-4(N-methylpyrrol-3-yl )-4-phenylbut-3--en-l-yl)nipecotic acid, 0 at N- (4-(-etyprrl- y14-hn bt-3-n y1)gvcie 0 20 N-(4-(furan-2--yl)-4-phenylbut-3-en-l-'yl)nipecotic acid, N- (furan-2-yl )-4-phenylbut-3-en-l-yl )guvacine, N-(4-(furan-2-yl)-4-phenylbut-3-en--l-yl)-O-homoproline, N-(4-(furan-3-yl)-4-phenylbut-3-el-l-yl)fipecotic acid, N-.(4-(furan-3-yl)-4-phenylbut-3--en-1-yl)guvacine, N-(4-(furan-3-yl)-4-phenylbut-3-en-1-yl)- -homoproline, N-(4-phenyl4-(pyridin-2-yl)but-3-en-1yl)lipecotic acid, N- (4-phenyl-4- (pyridin-2-yl )but-3-en-l-yl )guvacine, N-(4-phefyl-4-(pyridin-3-yl)but-3-efl-l-yl)nipecotic acid, N-(4-phenyl4-(pyridin-3yl)but3e'1-Y1)uvacie, N- (4-phenyl -4 -(pyridi.f-3 -yl but- 3-en- I-yl -6-homoprol ine, N-(4-phenYl-4-(pyridin-4-Yl)but-3-en--yl)liPecotic acid, N- (4-phenyl -4 -(pyridin-4 -yl) but- 3-el-l-yl) quvacine, N-(4-phenyl-4-(pyridin-4-yl)but-3-en-l -homoprlile, N -(4-phenyl-4-(pyrazin-2-yI)but-3-efl-1-yl)nipecotic acid, 4 TcN/VMN, 1986-12-16, 30, D-363, IL 3020,200 N- (4-phenyl-4- (pyrazin-2-y. )but-3-en-1-yl )guvaciner N- (4-phenyl-4- (pyrazin-2-yl )but-3-en-1-yl) -homoproline, N-(4-phenyl-4-(pyrazin-3-yl)but-3-en-1-yl)nipecotic ac.1.d, N-(4-phenyl-4-(pyrazin-3-yl)but-3-en-1-yl)guvac-ine, N-(4-phenyl-4-(pyrazin-3-y)but-3-en-1-y)--honoproline, N-(4-(l-rnethylimidazol-2-yl)-4-phenylbut-3-en-1-yl)nipecotic acid, N-(4-(l-methylimidazol-2-yl)-4-phenylbut-3-en-1-yl)guvacine, N- (4-(l-Iethylimidazol-2-yl)-4-phenylbut-3-en-1-yl)-Bhomoproline, 00 00 N-(4-(l-methylimidazol 4-y1)-4-phenylbut-3-en-1-y1)nipecotic 0O O 0 acid, -0 N-(4-(1-methylimidazol-4-yl)-4-phenylbut-3-en-1-yl)guvacine, 0015 honoproline, 1101o00 N-(4-(l-ntethylimidazol-5-yl)-4-phenylbut-3-en-1-yl)nipecotic 00000 acid, N-(4-(1-methylimidazol-5-y)-4-phenylbut-3-el-1-y)guvacifle, 0 N-(4-(l-methylimidazol-5-yi)-4-phenylbut-3-en-1-yl)-goi} ,20 homoproline, 0 N-(4-(2-methylphenyl)-4-(N-mfethylpyrrol-2-yl)but-3-elyl)nipecotic acid, N-(4-(2-methylphenyl)-4-(N-methylpyrrol-2-yl)btit-3-elyl)guvacifle, N-(4-(2-methylpheny)-4-(N-methylpyrrol-2-yl)but-3-en-1-yl)- hornopro line, N-(4-(2-methylphenyl)-4(Nfethylpyrrol-2-y1)but-3-efly1)nipecotic acid, N-(4-(2-nethylpheflyl)-4-(N-methylpyrrol>3yl)but-3-efl'>yl)guvacine, N-(4-(2-methylphenyl)-4-(N-methylpyrrol-3-yl)but-3-en-1-yl)-5hornopro line, N-(4-(2-methylphenyl)-4-(pyridiri-3-yl)but-2-en-1-yl)nipecotic acid, N-(4-(2-methylphenyl)-4-(pyridiin-3-y)l)but-2-en-1-yl)guvacine, ToN/VMN, 1986-12-16, 3o, D-363, IL 3020.200 N- (2-methyiphenyl) (pyridin-3-yl )but-2-en-1-yl) hornoproline, N- (2-methyiphenyl) (pyridin-3-yl )but-3-en-l-yl )nipecotic acid, N-(4-(2-methylphenyl)-4-(pyridin-3-yl)but-3-en-l-yl)guvacine, N(-2-methylphenyl)-4-(pyridin-3-yl)but-3-en-1-yl)-ghomopro line, N-(4-(N-rnethylpyrazol-3-yl)-4-phenylbut-3-en-1-yl)nipecotic acid, N-(4-(N-methylpyrazol-3-yl)-4-phenylbut-3-en-l-yl)guvacine, N-(4-(N-methylpyrazol-3-yl)-4-phenylbut-3-en-1-yl)-a- 0 homoproline, of N-methylpyrazol-4-yl)--4-phenylbut-3-en-l-yl)nipecotic 000000 acid, 0 0 00 15 N-(4-(N-rnethylpyrazol-4-yl)-4-phenylbut-3-en-l-yl)guvacine, o00 0 oN- (4-N-nethylpyrazol-4-yl -4-phenylbut-3-en-1-yl) 00000 homoproline, N- (N-methylpyrazol-S-yl) -4-phenylbut-3-en-1-yl )nipecotic 0n 0 0 acid, 0 004 0420 N-(4-(N-methylpyrazol-5-y1)-4-pheflb~ut->en-1-yl)guvacile, 0Of N-(4-(N-methy ,pyrazol15y)-4-phenlbut-3-efl-1-yl)- 000%homoproliie, 0 N-(4-(2-methylphelyl)-4-(N-mtethylpyrazol-3-yl)but-3-elyl )nipecotic acid, 0" 25 N-(4-(2-rnethylphefyl)-4-(N-methylpyrazol-3-y1)but-3-elyl )guvacine, N-(4-(2-tnethylphefyl)-4-(N-methylpyrazol-3-yl)but-3-efl-l-y1)- $-homoproline, N- (2-methyiphenyl) (N-nethylpyrazol-4-yl )but-3-en-lyl)nipecotic acid, N- (2-methyiphenyl )-4-(N-methylpyrazol-4-yl)but-3-en-1yl )guvacile, N-(4-(2-Inethylphefyl)-4-(N-methylpyrazol-4-yl)but-3-en-1-yl)- 0-homoproline, N-(4-(2-xnethylpbenyl)-4- (N-Inethylpyrazol-5-yl)but-3-nyJ.) nipecotic acid, 6 ToN/VMN, 1986-12-16, 3o, D-363, IL 3020.200 -methylphenyl)-4-( N-methylpyrazol-5 -yl)but- 3 en-lyl)guvacine, N-(4-(2-methylphenyl)-4-(N-methylpyrazol-5-y1)but-3-en-1-yl)a-homoproline,
N-(
4 2 -methylphenyl)-4-(-methylimidazol-2-yl)but-3-en-lyl)nipecotic acid,
N-(
4 2 -methylphenyl)-4-(l-methylimidazol-2-yl)but-3-en-lyl)guvacine, N- (4-(2-methylphenyl)-4- (l-methylimidazol-2-yl)but-3-en-1-yl) a-homoproline
N-(
4 3 -methyl-2-thienyl)-4-pheny1but-3-en-1-yl)nipecotic acid, 00 00 o N-( 4 -(3-methyl-2-th ienyl)-4-phenybut-3-en-1-yl)guvacine, oo0 N-( 4 -(3-methyl-2-thienyl)-4-phenylbut-3-en-l-yl)homoproline ooooo and salts thereof.
0 0 0o 15 Compounds of formula I may exist as geometric and o O optical isomers and all isomers and mixtures thereof are 0 00 00 0 0ooo included herein. Isomers may be separated by means of standard methods such as chromatographic techniques or fractional 00 crystallisation.
0 t 0 20 Cne embodiment of this invention is non-toxic o C pharmaceutically acceptable salts of compounds of formula I.
Salts include those derived from inorganic or organic acids such as hydrochloric, hydrobromic, sulfuric, phosphoric, acetic, lactic, maleic and phthalic acid.
Compounds of formula I may be prepared by Nalkylation of a compound of the general formula II H-R'3 (I) wherein R'3 has the same mraning as R 3 with the proviso that the carboxy group is protected, for example, by an ester group, with a compound of the general formula III 7 ToN/VMN, 1986-12-16, 3o, D-363, IL 3020.200 1 R -C=CH-CH 2
-CH
2
X
S(III)
2 1 2 wherein R and R are as defined in Claim 1, and X represents halogen. This reaction may be carried out in an inert solvent in the presence of an alkali metal carbonate, for example, potassium carbonate at, for example, room temperature, for from about 1 to 12 dys. The solvent may conveniently be acetone or N,N-dimethylformamide. Compounds of formula I may be prepared S 10 by hydrolysis of the resulting ester, preferably at room temperature in a mixture of an aqueous sodium hydroxide S°o, solution and an alcohol such as methanol or ethanol for from 0 oo.,o about 0.5 to 4 hours.
o o S oo Compounds of formula III may be prepared by reacting 0 000 0 oo 15 the appropriate disubstituted ketones with a Grignard reagent, i .o 00 cyclopropyl magnesium bromide, followed by ring opening of the intermediate cyclopropyl carbinol derivative by 0 treatment with hydrogen bromide in acetic acid. Alternative 0 00g o oe conditions involve the use of trimethylsilyl chlor.de and 0 Q0 lithium iodide in, for example, dichloromethane.
Sooao. Compounds of formula I are useful because they 0 possess pharmacological activity in man. In particular, the compounds of formula I are useful as inhibitors of GABA uptake.
0 For the above indications, the dosage will vary depending on the compound of formula I employed, on the mode of administration and on the therapy desired. However, in general, satisfactory results are obtained with a dosage of from about mg to about 2 g of compounds of formula I, conveniently given from 1 to 5 times daily, optionally in sustained release form. Usually, dosage forms suitable for oral administration comprise from about 25 mg to about 1 g of the compounds of formula I admixed with a pharmaceutical carrier or diluent. No toxic effects have been observed at these levels.
8 7 8 ToN/VMN, 1986-12-16, 30, D-363, IL 3020.200 The compounds of formula I may be administered in pharmaceutically acceptable acid addition salt form. Such acid addition salt forms exhibit approximately the same order of activity as the free base forms.
This invention also relates to pharmaceutical compositions comprising a compound of formula I or a pharmaceutically acceptable salt thereof and, usually, such compositions also contain a pharmaceutical carrier or diluent. The compositions of this invention may be prepared by conventional techniques to appear in conventional forms, for example, capsules or tablets.
a The pharmaceutical carrier employed may be conventional solid or liquid carriers. Examples of solid carriers are lactose, terra alba, sucrose, talc, gelatin, agar, pectin, oo .C acacia, magnesium stearate and stearic acid. Examples of liquid 15 carriers are syrup, peanut oil, olive oil and water. Similarly, go the carrier or diluent may include any time delay material well Oo known to the art, such as glyceryl monostearate or glyceryl distearate, alone or mixed with a wax.
If a solid carrier for oral administration is used, oO, 20 the preparation can be tabletted, placed in a hard gelatin capsule in powder or pellet form or in the form of a troche or ar. lozenge. The amount of solid carrier will vary widely but, usually, will be from about 25 mg to about 1 g. If a liquid carrier is used, the preparation may appear in the form of a S 25 syrup, emulsion, soft gelatin capsule or st-"ile injectable liquid such as an aqueous or non-aqueous liquid suspension.
The pharmaceutical compositions of this invention can be made following the conventional techniques of the pharmaceutical industry involving mixing, granulating and compressing or variously mixing and dissolving the ingredients as appropriate to give the desired and product.
The route of administration may be any route which effectively transports the active compound to the appropriate or desired place, such as orally or parenterally, the oral route being preferred.
A
ToN/VMN, 1986-12-16, 3o, D-363, IL 3020.200 The features disclosed in the foregoing description and in the following examples and claims may, both separately and in any combination thereof, be material for realising the invention in diverse forms thereof.
The process for preparing compounds of formula I and preparations containing them is further illustrated in the following examples, which, however are not to be construed as limiting. The examples illustrate some preferred embodiments.
Hereinafter T.l.c. is thin layer chromatography, THE is tetrahydrofuran and EtOH is ethanol.
o0 a Example 1 O2 o oo Cyclopropyl-(N-methylpyrrol-2-yl)phenylmethanol o a 9'00 *To a suspension of magnesium turnings (5,29 g, 0.22 molel in anhydrous tetrahydrofuran (70 ml), cyclopropyl bromide (26.35 g, 0.22 mole) in tetrahydrofuran (50 ml) was added dropwise under nitro-gn. The reaction mixture was heated at o" oreflux for one hoj, after the initial exotherm had subsided before N-methylpyrrol-2-ylphenylketone (13.3 g, 0.072 mole) (J.White and G. McGillivray, J.Org.Chem., (1977), 42, 4248, R.
Greenhouse and C. Ramirez, J.Org.Chem., (1985), 50, 2961) in anhydrous tetrahydrofuran (50 ml) was introduced dropwise.
After heating the reaction mixture at reflux for 3 hours it was cooled and saturated, aqueous ammonium chloride solution ml) and water (150 ml) were added. The mixture was extracted with ethyl acetate (3 x 200 ml) and the combined extracts were dried (MgSO4). Flash chromatography of the residue on evaporation on silica gel eluting with heptane/tetrahydrofuran provided the title compound as an oil (9.9 g, 46%) which solidified on standing. T.l.c. rf 0.35 (SiO 2 heptane/THF I, I TON/VMN, 1986-12-16, 3o, D-363, IL 3020.200 Ring opening of cyclopropylcarbinol: Method A Bromo-4-(N-methylpyrrol-2-yl)-4-phenylbut-3-ene Cyclopropyl-(N-methylpyrrol-2-yl)phenylmethanol was dissolved in acetic acid (60 ml) and a mixture of acetic acid (30 ml) and 48% hydrobromic acid (15 mi was added at 5 0 C. The mixture was stirred for 30 minutes and poured into water (300 ml). The resultant emulsion was extracted with ethyl acetate (2 x 100 ml). The combined organic layers were washed with saturated sodium bicarbonate solution and brine and dried (Na 2
SO
4 The concentrate, containing some acetic acid, was passed through a silica column (Merck Art 9385) with heptane/tetrahydrofuran (19:1) as eluent. After further flash chromatography in the same solvent system, the pure bromide (Z 00 0 o0 0 isomer) was obtained. T.l.c. rf 0.35 (Sio 2 heptane/THF o00oal5 00 0 0 000000 0 0 00 0 0 0 Method B Balmo, G. Fournet and J. Gore, Tetrahedron. Lett., 0 04 t: (1905), 1907 4-(N-Methylpyrrol-2-yl )-4-phenylbut-3-en-1-yl chloride and a iodide Cyclopropyl-(N-methylpyrrol-2-yl )phenyliethanol (6.46 g, 28.4 mmol) was dissolved in dichloromethane (200 ml) and lithium iodide (4.56 g, 31.4 mmol) was introduced. The mixture was cooled to 0 0 C, and chlorotrimethylsilane (3.6 ml# 28.4 mmol) was a:ied dropwise. After 2 hours at OOC, the reaction mixture was filtered and evaporated to a dark green oil (7.28 lash chromatoqgraphy on sil.ica gel (Merck Art 9385) eluting with heptane/tetrahydrofuran (19:1) provided the title compounds as an oil (6.3 g, 646) (a mixture of E and z isomers). T.I.c. rf t 0.29 (SiO 2 heptane/THPF ToN/VMN, 1986-12 1A. 3o, D-363, IL 3020 .200 (N-Methvlpyrrol-2-yl) -4-phenylbut-3-en-l-yl nipecotic acid ethyl ester 4- (N-Methylpyrrol-2-yl )-4-phenylbut-3-en-1-yl chloride and iodide (3.0 g, 8.7 minol)- were dissolved in anhydrous acetone (50 ml) and dried potassium ca-bonate (4.8 g, 34.8 mmol), sodium iodide (1.3 g, 8.7 mmol) and the Renantiomer of ethyl nipecotate (1,462 g, 9.3 rnmol) (A.M.
Akkerrnan et al., Rec.. Trav. Chem., 1951, 70, 899; G. Bettoni et al., Gazz. Chem. Ital. 1972, 102, 189) was added. The suspension was stirred at zoomn temperature for 10 days, r-'ltered and evaporated to a gummy residue which was puritied by flash chromatography on silica gel (Merck Art 9385). Elution with heptane/tetrahydrofuran (19:1) provided the title ester (1.74 0 0) 0" g, 54%) as an oil, TA c. rf 0.06 (SiQ hepte'ne/THF 0 0 00 0 o:0015 R-N- (4 -(N-Methylpyrro ,2 -y 1-4 -pheny lbut- 3-en 1-yl nipe cot ic 0 00 t acid hydrochloride (NO-05-0356) 0 a04 R -N i4- (N-Methylpyrro 1- 2-y1) -4 -pheny lbut 3-en ,l)nipecotic acid ethyl ester (1.74 g, 4.7 mmol) was dissolved 009 0 in ethanol (50 ml) and 10 N sodium hydroxide solution (8.9 ml) 0 20 was added. The solution was stirred at room temperature for miutes an'. cooled to 0 0 C. The pH was adjusted to 5 with 4 N hydrochloric acid solution, and the solution was extracted wtith dichlorome~hane (4 x 25 ml). The combined extracts were washed with water 110 ml) and dried (MgSO 4 The residue on evaporation was treated with water (100 ml) and activated charcoal. Filtration through a millipore filter gave a solution which was frezedried to give tche product as az cream solid (1,53 g, It was found that the E and Z isomers could be separated by kIPIC.
ToN/VMN, 1986-12-16, 3o, D-363, IL 3020.200 Example 2 N-(4-(N-Methylpyrrol-2-yl)-4-phenylbut-3-en-l-yl)nipecotic acid ethyl ester l-Bromo-4-(N-methylpyrrol-2-yl)-4-phenylbut-3-ene (4.58 g, 15.9 mmol) was dissolved in anhydrous acetone (115 ml) and dried potassium carbonate (8.78 g, 63.6 mmol) was introduced, followed by ethyl nipecotate (3.25 g, 20.7 mmol).
The reaction mixture was stirred at room temperature for 12 days, filtered and evaporated to give a brown oil (6.4 g), Column chromatography on silica gel (Merck Art 15111) eluting with heptane/tetrahydrofuran (19:1) provided the title compound as an oil (3.68 g, T.l.c. rf 0.31 (SiO 2 THF neptane 0 0 O o 0 00 0 o0ooo0 5 N-(4-N-Methylpyrrol-2-yl)-4-phenylbut-3-en-l-yl)nipecotic acid 0 hydrochloride (NO-05-0165) 0 0 0a o oI e N-(4-(N-Methylpyrrol-2-yl)-4-phenylbut-3-en-lyl)nipecotic acid ethyl ester (2.75 g, 7.5 aimol) was dissolved i o, in ethanol (70 ml). 10 N sodium hydroxide solution (14 ml) was I 20 introduced, and the solution was stirred for 30 minutes at room temperature before being cooled to 0°C. The pH was adjusted to 7 with 4 N hydrochloric acid solution, and the reaction mixture was extracted with dichlcromethane (4 x 100 ml) (emulsion). The combined organic extracts were washed with a mixture of saturated brine (20 ml) and water (20 ml). The layers were separated, and the aqueous phase was washed with dichloromethane (100 ml). The combined extracts were dried (Na 2
SO
4 and filtred through "hyflo". The filtrate was evaporated and the residue dissolved in 150 ml water, decolourised (charcoal) and freeze dried. The title amino acid was obtained as a dense white powder (Z isomer) (1.83 g, 72%).
T.l.c. rf 0.33 (SiO 2 dichloromethane/methanol r 13 ToN/VMN, 1986-12-16, 30, D-363, IL 3020.200 Example 3 2-Benzoyl-N-ethylpyrrole 2-Benzoylpyrrole (ref. as in Example 1) (10.27 g, 0.06 mole) was dissolved in dry N,N-dimethylformamide (120 ml) and combined with sodium hydride (2.016 g, 0.084 mole) (60% oil dispersion) in dry N,N-dimethylformamide (120 ml). The re&ation mixture was stirred at room temperature for 18 hours and water (100 ml) was added. The reaction mixture was extracted with diethyl ether (3 x 100 ml) and the combined extracts were washed with water (200 ml). The organic layer was dried (MgSO 4 g oo0 and evaporated to give the title compound as an oil (11.74 g, o 0 ooo T.1.c. rf 0.53 (SiO 2 dichloromethane/methanol 0o This ketone was converted into a mixture of 4-(N- 0 S15 ethylpyrrol-2-yl)-4-phenylbut-3-en-l-yl chloride and iodide by Oo 0 °oR the method described in Example 1 (using Method B) o Oa 0 0 R-N-((4-N-Ethylpyrr-l-2-yl)-4-pheylbut-3-en-l-yl)nipecotic acid ethyl ester 4-(N-Ethylpyrrol-2-yl)-4-phenylbut-3-en-l-yl chloride and iodide (3.16 g, 9 mmol) were dissolved in anhydrous acetone ml) and dried potassium carbonate (4.97 g, 36 mmol), sodium iodide (2.7 g, 18 mnmol) and the R-enantiomer of ethyl nipecotate (1.93 g, 13.7 mmol) were introduced. The suspension was stirred at room temperature for 10 days, filtered and evaporated to a residue. The residue was purified by column chromatography on silica gel (Merck Art 9385) eluting with heptane/tetrahydrofuran providing the title ester (1.50 g, 43%) as a gum. T.l.c. rf 0.21 (Si02, heptane/THF 14 ToN/VMN, 1986-12-1 6 30, D-363, IL 3020.200 4 -NEthylpyrrol-2-yl)-4-phenylbut-3-en-1-yl)nipecotic acid 4 -N-Ethylpyrrol-2-yl)-4-phenylbut-3-en-lyl)nipecotic acid ethyl ester (0.14 g, 0.4 mmol) was hydrolysed by the method outlined in Example 1. The title acid was obtained as a freeze-dried solid (Z isomer) (54 mg, m.p.
56.5 60 0 C (decomposition).
Example 4
N-(
4 -(N-Methylpyrrol-2-yl)-4-phenylbut-3-en-1-yl)guvacine methyl ester 0 0 co. 4- (N-Methylpyrrol-2-yl) -4 -phenylbut-3-en-l-yl Co 0 chloride and iodide (1.46 g, 4.3 mmol) (Example 1) were dissolved in anhydrous acetone (30 ml) and dried potassium o, carbonate (2.37 g, 17.2 mmol), sodium iodide (0.645 g, 4.3 o 15 mmol) and guvacine methyl ester hydrochloride. (0.995 g, 5.6 mmol) were added. The suspension was stirred at room temperature for 5 days, and worked up as described in Example 1 to give the title ester (1.1 g, 72%) as a fawn oil (mixture of E and Z isomers). T.l.c. rf 0.05 (Si02, heptane/THF N-(4-(N-Methylpyrrol-2-yl)-4-phenylbut-3-en-1-yl)guvacine hydrochloride (mixture of E and Z isomers) (NO-05-0387) N-(4-(N-(Methylpyrrol-2-yl)-4-phenylbut-3-en-lyl)guvacine (1.02 g, 2.9 mmol) was hydrolysed by the method outlined in Example 1. The title acid was obtained as a freeze dri6 solid (0.64 g, melting point: 81.5 84 0 C (E and Z isomers).
f, t ToN/VMN, 1986-12-16, 3o, D-363, IL 3020.200 N-(4-(N-Methylpyrrol-2-yl) -4-phenylbut-3-en-1-yl) guvacine methyl ester l-Bromo-4-(N-methylpyrrol-2-yl)-4-phenylbut-3-ene (0.60 g, 2.08 mmol) was dissolved in anhydrous acetone (20 ml) and dried potassium carbonate (1.10 g, 8 mmol) was introduced, followed by guvacine methyl ester hydrochloride (0.37 g, 2.08 mmol). The reaction mixture was stirred at room temperature for days and worked up as described in Example 1 to give the title ester (Z isomer) (380 mg, 52%) as an oil. T.l.c. rf 0.32 (Si02, heptane/THF N-(4-(N-Methylpyrrol-2-yl) -4-phenylbut-3-en-1-yl)guvacine hydrochloride (Z-isomer) N0-05-0227 0 i 0 N-(4-(N-Methylpyrrol-2-yl)-4-phenylbut-3-en-l- 0,o 06 0 a yl)guvacine methyl ester was hydrolysed by the method outlined 0 O'0 15 in Example 1. The title acid was obtained as a freeze dried on, white powder (60 mg, melting point: 70 0
C.
0 Example Cc clopropylphenyl- (4 -pyridyl) methanol Magnesium turnings (2.65 g, 0.109 mole) in dry tetrahydrofuran (50 ml) was treated dropwise with cyclopropyl bromide (13.2 ml, 0.109 mole). The reaction mixture was heated at reflux for 1 hour after the initial exotherm had subsided, and then 4-benzoylpyridine (10 g, 0.0545 mole) was introduced.
Heating at reflux was continued for 2 hours, the reaction mixture was cooled,and saturated ammonium chloride solution ml) was added. This aqueous phase was extracted with ethyl acetate (3 x 200 ml) and the combined extracts were dried (MgS04). Evaporation gave a crude solid residue (6.23 g) which 16 ToN/VMN, 1986-12-16, 3o, D-363, IL 3020.200 was recrystallized from toluene to give the title alcohol (2.57 g, m.p. 171 172 0 C. T.l.c. rf 0.065 (SiO 2 THF/heptane l-Bromo-4-phenyl-4-(4-pyridyl)but-3-ene Cyclopropylphenyl-4-(4-pyridyl)methanol (2.4 g, 10.6 mmol) was dissolved in acetic acid (25 ml). The solution was cooled to o0C. A 47% solution of hydrogen bromide (5 ml) was added and the reaction mixture was stirred at room temperature for 3.5 hours, and at 40 0 C for 1 hour. The reaction mixture was poured into water (100 ml) and this aqueous phase was extracted with ethyl acetate (3 x 50 ml). The combined organic extracts B on were washed with saturated sodium bicarbonate solution (40 ml) and saturated brine (40 ml) and dried (MgSO Evaporation gave "o0 a crude product (3.26 g) which was purified by flash a 15 chromatography on silica gel (Merck Art 9385). Elution with 0" heptane/ethyl acetate provided an oil (1.38 g, 45%) which solidified on standing. T.l.c. rf 0.13 (SiO 2 heptane/ethyl acetate N-(4-Phenyl-4-(4-pyridyl)but-3-en-l-yl)nipecotic acid, ethyl ester l-Bromo-4-phenyl-4-(4-pyridyl)but-3-ene (1.0 g, mmol), ethyl nipecotate 2 g, 4.6 mmol) and potassium carbonate (1.93 g, 14.0 nmlol) were stirred at room temperature for 5 days. The reaction mixture was filtered, and evaporated to a residue which was purified by flash chromatography on silica gel (Merck Art 9385). Elution with dichloromethane/ethanol/ 25 ammonium solution (190:9:1) provided the title compound as an oil. T.l.c. rf 0.23 (SiO 2
CH
2 C12/EtOH/NH 3 (190:9:1)).
e- 17 ToN/VMN, 1986-12-16, 3o, D-363, IL 3020.200 N-(4-Phenyl-4-(4-pyridyl)but-3-en-l-yl)nipecotic acid hydrochloride (N0-05-0358 N-(4-Phenyl-4-(4-pyridyl)but-3-en-l-yl)nipecotic acid ethyl ester was hydrolysed by the method outlined in Example 1.
The title acid was obtained as a freeze dried solid.
Example 6 Co oo 2-Methylphenyl-4-pyridylmethanol O 0 0000 Magnesium turnings (3.2 g, 0.131 mole) in dry 00o" tetrahydrofuran (50 ml) were treated dropwise with 2o o 10 bromotoluene (15 g, 0.087 mole). The reaction mixture was Qo oo o°00° heated at reflux for I hour after the initial reflux had 0000 subsided. After cooling, 4-pyridylcarboxaldehyde (14.38 g, 0,131 mole) in dry tetrahydrofuran (30 ml) was introduced 00 0oo, slowly, aind subsequently the reaction mixture was heated at o o" 15 reflux tor 2 hours. The reaction was worked up as in Example 0 O (Grignard reaction) to give the title alcohol (5.92 g, 34%).
0'0* T.l.c. rf 0.24 (SiO 2 ethyl acetate).
oI 4-(2-Methylbenzoyl)pyridine Pyridinium chlorochromate (9.29 g, 43.1 mmol) was dissolved in dichloromethane (50 ml) and a solution of 2methylphenyl-4-pyridylmethanol (5.72 g, 28.7 mmol) in dichloromethane (30 ml) was added. The reaction mixture became dark immediately, and was stirred for 2 hours at room temperature. Diethyl ether (350 ml) was added, and the reaction mixture was filtered through "hyflo" and evaporated to a dark oil (11.26 Flash chromatography on silica gel 'Merck Art I. I 18 ToN/VMN, 1986-12-16, 3o, D-363, IL 3020.200 9385) eluting with heptane/tetrahydrofuran provided the title compound (2.74 g, 48%) as an oil. T.l.c. rf 0.45 (SiO2' ethyl acetate).
This ketone was converted into l-bromo-4-(2methylphenyl)-4-(4-pyridyl)but-3-ene by the method described in Example 1 (Method A).
N-(4-(2-Methylphenyl)-4-(4-pyridyl)but-3-en-l-yl)nipecotic acid ethyl ester 00 0J, o0 o 0 0 l-Bromo-4-(2-methylphenyl)-4-(4-pyridyl)but-3-ene o J 10 (1.9 g, 7.6 mmol) was dissolved in anhydrous acetone (30 ml) and dried potassium carbonate (4.2 g, 30.4 mmol) and ethyl ooo mipecotate (2.39 g, 15.2 mmol) were introduced. The suspension o° was stirred at room temperature for 18 hours, filtered and oooo evaporated to a residue. The residue was purified by "flash" chromatography on silica gel (Merck Art 9385) eluting with 0ooo heptane/tetrahydrofuran to provide the title ester (0.67 oo g, 41%) as a reddish oil (a mixture of E and Z isomers). T.l.c.
0 0 rf 0.08 (Si02; heptane/THF N-(4-(2-Methylphenyl)-4-(4-pyridyl)but-3-en-1-yl)nipecotic acid N-(4-(2-Methylphenyl)-4-(4-pyridyl)but-3-en-lyl)nipecotic acid ethyl ester (0.67 g, 1.8 mmol) was dissolved in ethanol (20 ml) and 10 N sodium hydroxide solution (3.42 ml) was added. The solution was stirred at room temperature for Shours, and the pH was adjusted to 5 with 4 N hydrochloric acid.
The solution was applied to a column of Dowex 50WX8 ion exchange resin (H form). Elution with water followed by dilute ammonia solution provided the title acid (180 mg, fL .Itrtt 19 TON/VMN, 1986-12-16, 30, D-363, IL 3020.200 Example 7 2-Methylphenyl-(3-methyl-2-thienyl)methanol The title compound was prepared from 2-bromotoluene (35.55 g, 0.208 mole), magnesium turnings (5.1 g, 0.208 mole) and 3-methylthiophene-2-aldehyde (23.6 g, 0.187 mole) by the method described in Example 6, using diethyl ether (150 ml) as solvent. The yield was 36.0 g T.l.c. rf 0.39 (Sio 2 heptane/THF D0 00 00
OO
0 0000 0 0 0 1 3-Methyl-2-(2-methylbenzoyl)thiophene 0 000 00 0 0 00 Soo 10 2-Methylphenyl-(3-methyl-2-thienyl)methanol (36.0 g, 0 a 0.165 mole) was dissolved in dichloromethane (400 ml) and 0 "0 0o manganese dioxide (58 g, 0.667 mole) was added. The reaction mixture was heated at reflax for 18 hours, cooled and further 00 S"oo0 manganese dioxide (30 g, 0.34 mole) was introduced; reflux was 0o0 15 continued for a further 18 hours. The mixture was filtred and 0 00 evaporated to a residue (32 g) which was distilled in vacuo P (0.2 mm Hg). Fractions boiling at 100 120 0 C (4.8 g) and 120 132 0 C (21.0 g) were collected, giving the title compound as an oil (25.8 g, 72%).
The ketone was converted unto 1-bromo-4-(2methylphenyl)-4-(3-methyl-2-thienyl)but-3-ene by the method described in Example 1 (Method A) R-N-(4-12-Methylphenyl)-4-(3-methyl-2-ttienyl)but-3-en-lyl)nipecotic acid ethyl ester 1-Bromo-4- (2-methylphenyl)-4-(3-methyl-2thiinyl)but-3-ene (3.0 go 9.34 mmol) was dissolved in anhydrous acetone (40 ml) and dried potassium carbonate (1.38 g, 10 mmol) potassium iodide (0.2 g, 1 mmol) and the R-enantiomer of ethyl 1_1_1_ ToN/VMN, 1986-12-16, 30, D-363, IL 3020.200 nipecotate (1.57 g, 10 mmol' were introduced. The suspension was stirred at room temperature for 18 hours, filtered, and evaporated to a residue. The residue was purified by "flash" chromatography on silica gel (Merck Art 9385) eluting with heptane/tetrahydrofuran to provide tne title ester (2.4 g, 65%) as an oil. T.l.c. rf 0.40 (SiO 2 heptane/THF R-N-(4-(2-Methylphenyl)-4-(3-methyl-2-thienyl)but-3-en-lyl)nipecotic acid (NO-05-0340) 00 00 o 0 0 R-N-(4-(Z-Methylphenyl)-4-(3-methyl-2-thienyl)but-3- 000 oo 10 en-l-yl)nipecotic acid ethyl ester (1.4 g, 3.52 mmol) was "oo° hydrolysed by the method outlined in Example 1. The title acid Swas obtained as a solid (1.1 g, melting point: 65 67 0
C.
000o S0 9 Example 8 00 0 4 0 Cyclopropyl-2-furylphenylmethanol S 15 To a suspension of magnesium turnings (0.26 g, 10.5 mmol) in anhydrous tetrahydrofuran (6 ml) cyclopropyl bromide (1.28 g, 10.5 mmol) in tetrahydrofuran (5 ml) was added dropwise under nitrogen. The reaction mixture was heated at reflux for 1 hour after the initial exotherm had subsided before 2-benzoylfuran (12 g, 7.0 mmol) was added as a solution in tetrahydrofuran (10 ml). The reaction mixture was worked up as described in Example 1 to give the title alcohol as an oi.
T.l.c. rf 0.23 (SiO 2 heptane/THF This compound was converted directly into l-bromo-4- (2-furanyl)-4-phenylbut-3-ene by the method described in Example 1 (Method A).
cT 1 II.
I-
ToN/VMN, 1986-12-16, 3o, D-363, IL 3020.200 2 -Furanyl)-4-phenylbut-3-en-l-yl)nipecotic acid ethyl ester l-Bromo-4-(2-furanyl)-4-phenylbut-3-ene (0.23 g, 0.83 mmol) was dissolved in anhydrous acetone (10 ml) and dried potassium carbonate (0.46 g, 3.32 mmol) was added, followed by ethyl nipecotate (0.16 g, 1 mmol). The suspension was stirred at room temper.ture for 9 days, filtered and evaporated to a *residue. The residue was purified by column chromatography on silica gel (Merch Art 9385), eluting with heptane/tetrahydro- .0 furan to provide the title ester (140 mg, 47%) as an oil. T.l.c. rf 0.36 (SiO 2 heptane/THF N-(4-(2-Furanyl)-4-phenylbut-3-ene-l-yl)nipecotic acid N-(4-(2-Furanyl)-4-phenylb'it-3-en-l-yl)nipecotic acid ethyl ester (130 mg, 0.36 mmol) was hydrolysed by the method .5 described in Example 1. The title acid was obtained as a freeze dried solid. T.l.c. rf 0.43 (Sio,, methanol).
0 0 3 J 0 o a 3 3 0 0100o 00 0 a 0 0 Example 9 Preparation of Capsules.
Ingredients N-(4-(N-methylpyrrol-2yl)-4-phenylbut-3-en-l-yl)nipecotic acid Magnesium stearate Lactose Mg per Capsule 125 2 200 The above ingredients are thoroughly mixed and placed into hard gelatin capsules. Such capsules are administered orally to subjects in need of treatment from 1 5 times daily to enhance GABA'ergic activity in the central nervous system.
ToN/VMN, 1986-12-16, 3o, D-363, IL 3020.200 Example Preparation of Tablets.
Ingredients Mg per Tablet N-(4-(N-methylpyrrol-2yl)-4-phenylbut-3-en-l-yl)nipecotic acid 200 Corn starch 46 Polyvinyl pyrrolidone 12 Magnesium stearate 1 The compound is thorougaiy mixed with two thirds of the corn starch and granulated. The granules obtained are dried, mixed with the remaining ingredients and compressed into tablets.
The capsules or tablets thus prepared are administered orally. Similarly, other compounds of formula I can be used.
00 0 0 0 0 10 S0 0 a 0 O 0 0I00 0 0 0 00 0 0 0 0ow PHARMACOLOGICAL T3ST introduction The convulsions induced by loud noise in the DBA/2 strain of mice is regarded as a reliable model fnr evaluating antiepileptic drug effects, cf. E.N. Petersen et al.: psychopharmacol, 83 (1984), 240, and A.G. Chapman et al.: Arzmeim.-Forsch. 10 (1984), 1261. The Rotarod and Traction tests were used to evaluate the sedative properties of the test drugs.
Methods Male DBA/2 mice (8 1 g) were used in all experiments. The animals were pretrained on the Rotarod (6 rpm; rod diameter 2.5 cm) for 1 minute. The compoinds tested were injected intraperitoneally. Twenty-five minutes later, the 23 ToN/VMN, 1986-12-16, 3o, D-363, IL 3020.200 animals underwent a 2 minutes' test on the Rotarod. The number of failures to stay on the rod was counted. An error rate higher than 10 was assigned the maximum score of Immediately after the Rotarod test, the animals were tested in a Traction test, cf. Psychopharmacol. above. In this test, the animal was required to maintain grasp on a thin rod (diameter mm) with the forepaws for five seconds and, within this period of time, to show a traction response (grasping onto the rod with one of the hindlcys). The performance on the test was based on the absence or presence of the traction response with the 5 seconds' test period. Finally, after the Traction test, o the animals were individually placed in a chamber in which they o were exposed for 30 seconds to a 14 kHz sinus tone at 111 dB.
on During this period of time, the following behaviors were noted: i 15 K.'ild running", clonic convulsions and death.
S 0 0 00 Drugs 0 The compounds tested were dissolved in distilled i o water or suspended in 5% chremophore. The injection volume was 0.2 ml/mouse.
0 Results obtained g* In table I, below, th- ratio ED 50 Rotarod/ED 50 tonic convulsions is given for the compounds tested. NO-05-0340 is R-N-(4-(2-methy' henyl)-4-(3-methyl-2-thienyl)but-3-en-lyl)nipecotic acid and NO-05-0356 is R-N-(4-(N-methylpyrrol-2yl)-4-phenylbut-3-en-1-yl)nipecotic acid.
1, 0 ToN/VMN, 1986-12-16, 30, D-363, IL 3020.200C Table I Comp~ound- NO-05-0340 -03 56 SK&F 1OU330A SK&F 89976A SK&F 100561 Ratio 0 0 0 0 0 0 0 0 0 0 0 0 00

Claims (17)

1. Phenylbuten derivatives of the general formula I R -C=CH-CH2-CH2-R 3 22 R wherein R 1 represents phenyl optionally substituted by one, two or more substituents selected from the group consisting of halogen, lower alkyl, and lower alk.xy, R2 represents pyrrolyl, furany', pvridinyl pyrazinyl, imidazolyl pyrazolyl, pyrimidinyl pyrrolldinyl, tetrahydrofuranyl, piperidinyl or piperazinyl each of which may be subs~ituted by one, two or more substituents selected from the group consisting of halogen, lower alkyl and lower alkoxy or R2 represents a thienyl group substituted by a loweralkyl group which substituted thienyl group may be further substituted by one, two or more substituents selected from the group consisting of halogen, lower alkyl, and lower alkoxy, and R represents
3-carboxypiperid-l-yl 3-carboxy-l,2,5,6-tetrahydropyrid--yl or 3-carboxymethylIpyrrolidin-l-yl, the corresponding amides or lower alkyl esters, or salts thereof. 2. Derivatives, according -to Claim 1, characterized in that R3 is 3-carboxypiperid-l-yl or 3-carboxy-1 2,5,6-tetrahydropyrld-l-yl, 3, Derivatives, according to Claim 1 or 2, characterized in that R 2 represents pyrrolyl, furanyl, pyridinyl, pyrazinyl, imilazolyl, pyrazolyl pyrimidinyl tetrahydrofuranyl piperidinyl or thienyl substituted by a lower alkyl group, each of which i y be substituted by one, two or more substituents selected from the group consisting of halogen, lower alkyl, and lower alkoxy.
4. Derivatives, according to any one of the preceding claims, wherein R2 is 2-pyrrolyl, Derivatives, according to any one of the Claims 1 through 3, wherein R 2 Is 2-furanyl.
6. DerivatIves, according to any one of the C'ialms 1 through 3, wherein R2 Is 2-imidazolyl.
7. DerivatIves, according to any one of the Claims 1 through 3, wherein R 2 is N-methylpyrazolyl.
8. Derivatives, according to any one of the Claims 1 through 3, wherein R2 is 5-pyrimidinyl.
11. 3-methylthi
12. characteriz methyl, eth
13. characteriz alkyl.
14. methyl, eth wherein R
16. stated in a carrier, di
17. r> contain fro >i o 18. patient, wh' said increa at least a composition
19. or a salt t formula IV wherein R converting z into a comp(
20. 1 herein descr
21. P described wI 22, a patient, 1 ,3WBSl Kk 8511U 26 11. Derivatives, according to Claim 9 or Claim 10, wherein R 2 is 3-methylthien-2-yl. 12. Derivatives, according to any one of the Claims 1 through 3, characterized in that R is phenyl substituted by chloro, bromo, fluoro, methyl, ethyl or methoxy. 13. Derivatives, according to any one of the Claims 1 through 3, characterized in that the heterocyclic group is substituted with lower alkyl. 14. Derivatives, according to Claim 13, wherein the lower alkyl is methyl, ethyl, isopropyl or propyl. Derivatives, according to any one of the Claims 1 through 3, wherein R 2 is N-methylpyrrol-2-yl. 16. Pharmaceutical compositions containing a compound of formula I stated in any one of the preceding claims or a salt thereof together with a oo carrier, diluent and/or excipient. 17. Compositions, according to Claim 16, characterized in that they contain from about 25 mg to about 1 g of the compound. o 18. A method for increasing GABA'ergic activity and/or sedating a o°u patient, which method comprises administering to said patient requiring I said increase in GABA'ergic activity and/or sedation an effective amount of at least a derivative according to any one of Claims 1 to 15 or a composition according to Claim 16 or Claim 17. 19. A process for preparing compounds of formula I stated in Claim 1 S or a salt thereof, characterized in hydrolysirg a compound of the general formula IV S. R 1 -C=CH-CH -CH R 13 (IV) S12 R wherein R 1 R 2 and R' 3 each are as defined above, and, if desired, converting a compound of formula I into a salt thereof or converting a salt into a compound of formula I. A N-(butenyl-substituted)azaheterocyclic carboxylic acid as herein described with reference to any one of Examples 1 to 8. 21. A pharmaceutical composition, substantially as hereinbefore described with reference to Example 9 or Example
22. A method for increasing the GABA'ergic activity and/or spating a patient, which method comprises administering to said patient requ. J 0/7 511U h M^y J t .r r *i ;r fs^E.-F- 27 said increase in GABA'ergic activity and/or sedation an effective amount of a derivative according to Claim 20 or a composition according to Claim 21.
23. A process for preparing a N-(butenyl-substituted)azaheterocyclic carboxylic acid, substantially as hereinbefore described with reference to any one of Examples 1 to 8. DATED this FOURTH day of MAY 1990 Novo Industri A/S Patent Attorneys for the Applicant SPRUSON FERGUSON
AU67193/87A 1986-01-07 1987-01-07 N- (butenyl-substituted) azaheterocyclic carboxylic acids Ceased AU600248B2 (en)

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DK704488D0 (en) * 1988-12-19 1988-12-19 Novo Industri As NEW N-SUBSTITUTED AZAHETEROCYCLIC CARBOXYLIC ACIDS
DK288385D0 (en) * 1985-06-26 1985-06-26 Novo Industri As AMINO ACID DERIVATIVES
DK270488D0 (en) * 1988-05-18 1988-05-18 Novo Industri As Hitherto unknown O-SUBSTITUTED KETOXIMES
DK588189D0 (en) * 1989-11-22 1989-11-22 Novo Nordisk As NEW HETEROCYCLIC CARBOXYLIC ACIDS
US5112980A (en) * 1989-12-27 1992-05-12 Monsanto Company Process of preparing substituted pyridine compounds
US5962449A (en) 1995-04-07 1999-10-05 Novo Nordisk A/S Tricyclic compounds in treating hyperalgesic conditions and NIDDM
US6191165B1 (en) * 1996-05-31 2001-02-20 Allelix Neuroscience Inc. Pharmaceutical for treatment of neurological and neuropsychiatric disorders
WO1997049403A1 (en) * 1996-06-27 1997-12-31 University College Dublin Use of nipecotic acid or guvacine derivatives for the manufacture of a medicament for the treatment of postischemic neurodegenerative disorders
US6503926B2 (en) 1998-09-04 2003-01-07 Millennium Pharmaceuticals, Inc. Chemokine receptor antagonists and methods of use therefor
US6288083B1 (en) 1998-09-04 2001-09-11 Millennium Pharmaceuticals, Inc. Chemokine receptor antagonists and methods of use therefor
DE19840611A1 (en) * 1998-09-05 2000-03-09 Klaus Wanner GABA uptake inhibitors with pyrrolidine structure
HRP20030696A2 (en) 2001-02-16 2005-04-30 NPS Allelix Corp. Allelix Neuroscience GlyT-1 INHIBITORS
US7355042B2 (en) * 2001-10-16 2008-04-08 Hypnion, Inc. Treatment of CNS disorders using CNS target modulators
US7189757B2 (en) * 2001-10-16 2007-03-13 Hypnion, Inc. Treatment of sleep disorders using CNS target modulators
WO2003032912A2 (en) * 2001-10-16 2003-04-24 Hypnion, Inc. Treatment of cns disorders using cns target modulators
CN1382441A (en) * 2002-05-21 2002-12-04 中国科学院上海生命科学研究院 Application of gammalon transporter inhibitor in preparing analgesic

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FI89481B (en) 1993-06-30
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US4931450A (en) 1990-06-05
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IL81179A0 (en) 1987-08-31
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DK165692B (en) 1993-01-04

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